One-step oxidation of benzene to phenol with H3PW12O40 under photoirradiation: Effect of operating conditions

نویسندگان

چکیده

The synthesis of phenol by one-pot oxidation benzene with dioxygen (O2) is a significant conceptual and practical challenge because has low reactivity to O2 at room temperature ambient pressure. Furthermore, more reactive than easily overoxidized, so complete likely proceed in the reaction, which generally results lower yield selectivity. Herein, we report that heteropolyacid H3PW12O40 functions as photocatalyst for reaction an aqueous acetonitrile solution using high (23–41%) selectivity (80–90%). addition significantly inhibited complexation between H3PW12O40, preventing overoxidation. no decomposition during was evidenced UV–VIS spectra. This can be used repeatedly only slight decrease rate formation. For mechanistic study, initial rates, depended on conditions, were investigated detail. under anaerobic conditions also conducted control experiment. A color change from colorless blue confirmed reduction catalytic process formation reduced detected kinetic isotope effect (KIE), kH/kD = 1.15, found benzene/benzene‑d6, indicating electron transfer principal C−H bond activation mechanism. We identified hydrogen peroxide intermediate generated both photocatalytic reoxidation our system.

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ژورنال

عنوان ژورنال: Chemical Engineering Journal

سال: 2022

ISSN: ['1873-3212', '1385-8947']

DOI: https://doi.org/10.1016/j.cej.2021.131369